A comparative study of different exchange-correlation functionals in understanding structural, electronic and thermoelectric properties of Fe$_{2}$VAl and Fe$_{2}$TiSn compounds

TL;DR

This study compares various exchange-correlation functionals in density functional theory to evaluate their effectiveness in predicting the structural, electronic, and thermoelectric properties of Fe$_{2}$VAl and Fe$_{2}$TiSn full Heusler compounds.

Contribution

It systematically assesses five different functionals, including recent ones like PBEsol, mBJ, and SCAN, for their accuracy in modeling these thermoelectric materials.

Findings

mBJ functional predicts band gaps close to experimental values

Fe$_{2}$VAl is semimetallic with negative gaps from most functionals

Fe$_{2}$TiSn shows semimetallic or semiconducting behavior depending on the functional

Abstract

Fe$_{2}$VAl and Fe$_{2}$TiSn are full Heusler compounds with non-magnetic ground state. The two compouds are good thermoelectric materials. PBE and LDA(PW92) are the two most commonly used density functionals to study the Heusler compounds. Along with these two well studied exchange-correlation functionals, recently developed PBEsol, mBJ and SCAN functionals are employed to study the two compounds. Using the five functionals equilibrium lattice parameter and bulk modulus are calculated. Obtained values are compared with experimental reports wherever available. Electronic structure properties are studied by calculating dispersion curves, total and partial density of states. For Fe$_{2}$VAl, band gap of 0.22 eV is obtained from the mBJ potential which is in reasonable agreement with experimental value while, for Fe$_{2}$TiSn band gap of 0.68 eV is obtained. Fe$_{2}$VAl is predicted to be semimetallic with different values of negative gaps from LDA,PBEsol,PBE and SCAN functionals. Whereas, Fe$_{2}$TiSn is found to be semimetallic(semiconducting) from LDA,PBEsol(PBE,SCAN) functionals employed calculations. From the dispersion curve effective mass values are also computed to see the contribution to the Seebeck coefficient. In Fe$_{2}$TiSn, a flat band is present along the $\Gamma$-X direction with calculated value of effective mass $\sim$36 more than the mass of electron. The improvements or inadequacies among the functionals in explaining the properties of full Heusler alloys for thermoelectric application are thus observed through this study.